用智能算法仅需15-20%数据点,精准重建X射线谱图。
Demonstration of an AI-driven workflow for dynamic x-ray spectroscopy
- 注入领域知识的贝叶斯优化,自动识别吸收边和前峰特征。
- 用15-20%采样点实现亚0.1 eV吸收边精度,误差低于0.03 eV。
- 适合电池、催化剂等动态化学过程研究,提升实验效率与时间分辨率。
X射线吸收近边结构(XANES)光谱可精准刻画材料中元素的化学态与对称性,但需在多个能量点采集数据,耗时较长。现有自适应采样方法常缺乏对XANES谱结构的领域知识。本文提出一种融合谱图特征(如吸收边、前峰)知识的贝叶斯优化方法,实现高效自适应采样。实验表明,该方法仅需常规采样点的15-20%,即可准确重构吸收边,且吸收边误差小于0.1 eV,尖峰能量误差小于0.03 eV,整体均方根误差小于0.005。在电池材料与催化剂上的测试验证了其在静态与动态测量中的有效性,显著提升数据采集效率,支持高时间分辨率追踪化学演变。该方法提升了XANES实验自动化水平,减少近吸收边区域的过采样或欠采样问题,适用于受限测量时间或需高时序解析的场景。
原文摘要 · Abstract (English)
X-ray absorption near edge structure (XANES) spectroscopy is a powerful technique for characterizing the chemical state and symmetry of individual elements within materials, but requires collecting data at many energy points which can be time-consuming. While adaptive sampling methods exist for efficiently collecting spectroscopic data, they often lack domain-specific knowledge about XANES spectra structure. Here we demonstrate a knowledge-injected Bayesian optimization approach for adaptive XANES data collection that incorporates understanding of spectral features like absorption edges and pre-edge peaks. We show this method accurately reconstructs the absorption edge of XANES spectra using only 15-20% of the measurement points typically needed for conventional sampling, while maintaining the ability to determine the x-ray energy of the sharp peak after absorption edge with errors less than 0.03 eV, the absorption edge with errors less than 0.1 eV; and overall root-mean-square errors less than 0.005 compared to compared to traditionally sampled spectra. Our experiments on battery materials and catalysts demonstrate the method's effectiveness for both static and dynamic XANES measurements, improving data collection efficiency and enabling better time resolution for tracking chemical changes. This approach advances the degree of automation in XANES experiments reducing the common errors of under- or over-sampling points in near the absorption edge and enabling dynamic experiments that require high temporal resolution or limited measurement time.
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